Science Advances

Supplementary Materials

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  • Supplementary Materials and Methods
  • Supplementary Text
  • Fig. S1. PXRD of SIFSIX-18-Ni.
  • Fig. S2. Variable temperature PXRD of SIFSIX-18-Ni.
  • Fig. S3. Comparison of experimental PXRD profiles for SIFSIX-18-Ni-α, SIFSIX-18-Ni-β, and SIFSIX-18-Ni-γ with their calculated patterns and related polymorphs (24) (all recorded at 298 K).
  • Fig. S4. Comparison of experimental PXRD profiles for SIFSIX-18-Ni-β, SIFSIX-18-Ni-β (activated, before dosing CO2), and SIFSIX-18-Ni-β (dosed with 1 bar CO2 at 303 K) with the calculated pattern of SIFSIX-18-Ni-β.
  • Fig. S5. Comparison of experimental PXRD profiles for SIFSIX-18-Ni-α, SIFSIX-18-Ni-β, and SIFSIX-18-Ni-β (activated, before dosing H2O).
  • Fig. S6. Particle size distribution around the mean diameter (~13.94 μm) range of SIFSIX-18-Ni-β.
  • Fig. S7. Thermogravimetric analysis profiles of SIFSIX-18-Ni.
  • Fig. S8. CO2 sorption isotherms for SIFSIX-18-Ni-β; inset: low pressure range until 0.01 bar.
  • Fig. S9. Low-temperature CO2, N2, and O2 sorption isotherms for SIFSIX-18-Ni-β.
  • Fig. S10. CO2 and N2 sorption isotherms for SIFSIX-18-Ni-β.
  • Fig. S11. CO2 and O2 sorption isotherms for SIFSIX-18-Ni-β.
  • Fig. S12. CO2 sorption isotherms at 298 K for SIFSIX-18-Ni-α (only subjected to evacuation after MeOH washing of precursor, i.e., no heating), SIFSIX-18-Ni-β, and SIFSIX-18-Ni-γ.
  • Fig. S13. CO2 and N2 sorption isotherms for Mg-MOF-74.
  • Fig. S14. CO2 and N2 sorption isotherms for Zeolite 13X.
  • Fig. S15. CO2 and N2 sorption isotherms for SIFSIX-3-Ni.
  • Fig. S16. CO2 and N2 sorption isotherms for NbOFFIVE-1-Ni.
  • Fig. S17. CO2 and N2 sorption isotherms for TIFSIX-3-Ni.
  • Fig. S18. CO2 and N2 sorption isotherms for ZIF-8.
  • Fig. S19. Fitting of the isotherm data for SIFSIX-18-Ni-β to the virial equation.
  • Fig. S20. Fitting of the isotherm data for ZIF-8 to the virial equation.
  • Fig. S21. H2O sorption isotherms for SIFSIX-18-Ni-β compared with other HUMs (all recorded at 298 K).
  • Fig. S22. Sorption isotherms (298 K) for CO2 and H2O for SIFSIX-18-Ni-β compared with other HUMs; pressure range until 0.03 bar i.e. saturation pressure of H2O at 298 K.
  • Fig. S23. H2O sorption isotherms (298 K) of SIFSIX-18-Ni-β for vacuum DVS and intrinsic DVS experiments.
  • Fig. S24. H2O sorption isotherms of SIFSIX-18-Ni-β recorded at different temperatures by intrinsic DVS experiments.
  • Fig. S25. Humidity-dependent CO2/H2O selectivities (SCW) for SIFSIX-18-Ni-β at 298 K.
  • Fig. S26. CO2/H2O selectivities (SCW) for SIFSIX-18-Ni-β under different CO2 concentrations at 298 K.
  • Fig. S27. 0.1/99.9 (v/v) CO2/N2 breakthrough profiles and CO2 effluent purities for SIFSIX-18-Ni-b under dry and 74% RH conditions; flow rate = 20 cm3 min−1.
  • Fig. S28. 0.3/99.7 (v/v) CO2/N2 breakthrough profiles and CO2 effluent purities for SIFSIX-18-Ni-b under dry and 74% RH conditions; flow rate = 20 cm3 min−1.
  • Fig. S29. 0.1/99.9 (v/v) CO2/N2 breakthrough profiles and CO2 effluent purities for NbOFFIVE-1-Ni under dry and 74% RH conditions; flow rate = 20 cm3 min−1.
  • Fig. S30. 0.3/99.7 (v/v) CO2/N2 breakthrough profiles and CO2 effluent purities for NbOFFIVE-1-Ni under dry and 74% RH conditions; flow rate = 20 cm3 min−1.
  • Fig. S31. 0.1/99.9 (v/v) CO2/N2 breakthrough profiles and CO2 effluent purities for Zeolite 13X under dry and 74% RH conditions; flow rate = 20 cm3 min−1.
  • Fig. S32. 0.3/99.7 (v/v) CO2/N2 breakthrough profiles and CO2 effluent purities for Zeolite 13X under dry and 74% RH conditions; flow rate = 20 cm3 min−1.
  • Fig. S33. 0.1/99.9 (v/v) CO2/N2 breakthrough profiles and CO2 effluent purities for SIFSIX-3-Ni under dry and 74% RH conditions; flow rate = 20 cm3 min−1.
  • Fig. S34. 0.3/99.7 (v/v) CO2/N2 breakthrough profiles and CO2 effluent purities for SIFSIX-3-Ni under dry and 74% RH conditions; flow rate = 20 cm3 min−1.
  • Fig. S35. 0.1/99.9 (v/v) CO2/N2 breakthrough profiles and CO2 effluent purities for TIFSIX-3-Ni under dry and 74% RH conditions; flow rate = 20 cm3 min−1.
  • Fig. S36. 0.3/99.7 (v/v) CO2/N2 breakthrough profiles and CO2 effluent purities for TIFSIX-3-Ni under dry and 74% RH conditions; flow rate = 20 cm3 min−1.
  • Fig. S37. 1000 ppm CO2/N2 (v/v = 0.1/99.9%) breakthrough profiles for ZIF-8 under dry condition, flow rate = 20 cm3 min−1.
  • Fig. S38. 3000 ppm CO2/N2 (v/v = 0.3/99.7%) breakthrough profiles for ZIF-8 under dry condition, flow rate = 20 cm3 min−1.
  • Fig. S39. 0.5/99.5 (v/v) CO2/N2 breakthrough profiles and CO2 effluent purities for SIFSIX-18-Ni-β and NbOFFIVE-1-Ni under dry and 74% RH conditions; flow rate = 10 cm3 min−1.
  • Fig. S40. 1/99 (v/v) CO2/N2 breakthrough profiles and CO2 effluent purities for SIFSIX-18-Ni-β and NbOFFIVE-1-Ni under dry and 74% RH conditions; flow rate = 10 cm3 min−1.
  • Fig. S41. Temperature‐programmed desorption plot of DAC of CO2 experiment for SIFSIX-18-Ni-β.
  • Fig. S42. PXRD profiles for SIFSIX-18-Ni before and after accelerated stability test.
  • Fig. S43. BET surface areas as obtained from 77 K N2 adsorption isotherms for SIFSIX-18-Ni and other adsorbents, after accelerated stability test.
  • Fig. S44. CO2 adsorption isotherms (298 K) for SIFSIX-18-Ni after accelerated stability test.
  • Fig. S45. IAST selectivity comparison for benchmark physisorbents at CO2 (500 ppm): N2 binary mixture; results for SIFSIX-18-Ni-β not included as partial sieving effect is observed.
  • Fig. S46. IAST selectivities found in SIFSIX-18-Ni-β for CO2/O2 binary mixtures with varying CO2 concentrations.
  • Fig. S47. FTIR spectra of SIFSIX-18-Ni: as-synthesized, activated (β), after CO2 sorption, after H2O sorption, and after 1-hour CO2 dosing at 1 bar.
  • Fig. S48. 0.1/99.9 (v/v) CO2/N2 adsorption-desorption recyclability over 6 consecutive cycles for SIFSIX-18-Ni-β under dry and 74% RH conditions.
  • Fig. S49. 0.3/99.7 (v/v) CO2/N2 adsorption-desorption recyclability over 6 consecutive cycles for SIFSIX-18-Ni-β under dry and 74% RH conditions.
  • Fig. S50. 0.5/99.5 (v/v) CO2/N2 adsorption-desorption recyclability over 6 consecutive cycles for SIFSIX-18-Ni-β under dry and 74% RH conditions.
  • Fig. S51. 1/99 (v/v) CO2/N2 adsorption-desorption recyclability over 6 consecutive cycles for SIFSIX-18-Ni-β under dry and 74% RH conditions.
  • Fig. S52. CO2 adsorption-desorption recyclability over 100 cycles for SIFSIX-18-Ni-β (1.0 bar CO2; desorption at 348 K): for each cycle, 60 min of isothermal (303 K) gravimetric CO2 uptake recorded on the activated sample.
  • Fig. S53. Comparison of gravimetric C-capture kinetics in SIFSIX-18-Ni-β and TEPA-SBA-15 under dry conditions.
  • Fig. S54. Comparison of gravimetric C-capture kinetics in SIFSIX-18-Ni-β and TEPA-SBA-15 under wet conditions.
  • Fig. S55. Diffractograms for the Le Bail refinement of SIFSIX-18-Ni-α.
  • Fig. S56. Diffractograms for the Rietveld refinement of SIFSIX-18-Ni-β.
  • Fig. S57. Equilibrated structure of CO2 molecules residing in the cavity of SIFSIX-18-Ni-β corresponding to a loading of 2 CO2 per formula unit.
  • Fig. S58. Scheme of the coupled gas mixing system, TGA-based gas uptake analysis, and breakthrough separation analysis unit.
  • Table S1. Calculated SCW at 74% RH.
  • Table S2. Fitting parameters for SIFSIX-18-Ni-β.
  • Table S3. Fitting parameters for ZIF-8.
  • Table S4. Dynamic breakthrough experiment details of CO2/N2 at 298 K and 1 bar.
  • Table S5. Crystallographic data for SIFSIX-18-Ni.
  • References (4145)

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